Second-Order Nonlinear Optics from First Principles

TL;DR

This paper introduces a first-principles theoretical approach based on Time-Dependent Density-Functional Theory to accurately calculate second-order nonlinear optical properties, including many-body effects, demonstrated on GaAs.

Contribution

A novel first-principles method for calculating second-order susceptibility using TDDFT that incorporates many-body effects.

Findings

Accurately predicts Second-Harmonic Generation spectra for GaAs

Shows excellent agreement with experimental data

Provides a practical framework for nonlinear optical property calculations

Abstract

We present a new first-principle theory for the calculation of the macroscopic second-order susceptibility chi^(2), based on the Time-Dependent Density-Functional Theory approach. Our method allows to include straightforwardly the many-body effects. We apply the theory to the computation of the Second-Harmonic Generation spectroscopy, showing a very good agreement with experiment for cubic semiconductor GaAs.